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Increasing impacts of wildfires on Western US air quality highlights the need for forecasts of smoke emissions based on dynamic modeled wildfires. This work utilizes knowledge of weather, fuels, topography, and firefighting, combined with machine learning and other statistical methods, to generate 1‐ and 2‐day forecasts of fire radiative energy (FRE). The models are trained on data covering 2019 and 2021 and evaluated on data for 2020. For the 1‐day (2‐day) forecasts, the random forest model shows the most skill, explaining 48% (25%) of the variance in observed daily FRE when trained on all available predictors compared to the 2% (<0%) of variance explained by persistence for the extreme fire year of 2020. The random forest model also shows improved skill in forecasting day‐to‐day increases and decreases in FRE, with 28% (39%) of observed increase (decrease) days predicted, and increase (decrease) days are identified with 62% (60%) accuracy. Error in the random forest increases with FRE, and the random forest tends toward persistence under severe fire weather. Sensitivity analysis shows that near‐surface weather and the latest observed FRE contribute the most to the skill of the model. When the random forest model was trained on subsets of the training data produced by agencies (e.g., the Canadian or US Forest Services), comparable if not better performance was achieved (1‐day R2 = 0.39–0.48, 2‐day R2 = 0.13–0.34). FRE is used to compute emissions, so these results demonstrate potential for improved fire emissions forecasts for air quality models. Plain Language Summary: Increasing wildfire smoke is undoing decades of air quality progress, yet air quality forecasts often miss the most intense smoke events. This is because forecasted smoke is released at constant rates whereas the rate of smoke release from real wildfires varies in time. In this work we teach a machine learning algorithm to predict the daily change in fire heat output, a quantity that is used to calculate wildfire emissions. The machine learning algorithm uses information regarding weather, fuel moisture and amount, and firefighting efforts to make its predictions. We also tried to predict the daily change in fire heat output using only weather information but found the machine learning method to be more successful. Many federal agencies have their own ways of tracking fire weather and fuel moisture, and in this paper, we show that we can apply machine learning to the data from any of several agencies and get the same level of forecasting skill. Key Points: Random forest models trained on weather, fuel, and firefighting data surpass persistence and weather‐based methods to predict fire energyRandom forest models beat persistence across states, for most days in the 2020 fire season, and across levels of fire severityFire weather and latest fire energy predictors add most skill to the random forest; models using agency weather data perform similarly [ABSTRACT FROM AUTHOR]

Predicting the evolution of burned area, smoke emissions, and energy release from wildfires is crucial to air quality forecasting and emergency response planning yet has long posed a significant scientific challenge. Here we compare predictions of burned area and fire radiative power from the coupled weather/fire‐spread model WRF‐Fire (Weather and Research Forecasting Tool with fire code), against simpler methods typically used in air quality forecasts. We choose the 2019 Williams Flats Fire as our test case due to a wealth of observations and ignite the fire on different days and under different configurations. Using a novel re‐gridding scheme, we compare WRF‐Fire's heat output to geostationary satellite data at 1‐hr temporal resolution. We also evaluate WRF‐Fire's time‐resolved burned area against high‐resolution imaging from the National Infrared Operations aircraft data. Results indicate that for this study, accounting for containment efforts in WRF‐Fire simulations makes the biggest difference in achieving accurate results for daily burned area predictions. When incorporating novel containment line inputs, fuel density increases, and fuel moisture observations into the model, the error in average daily burned area is 30% lower than persistence forecasting over a 5‐day forecast. Prescribed diurnal cycles and those resolved by WRF‐Fire simulations show a phase offset of at least an hour ahead of observations, likely indicating the need for dynamic fuel moisture schemes. This work shows that with proper configuration and input data, coupled weather/fire‐spread modeling has the potential to improve smoke emission forecasts. Plain Language Summary: Predicting wildfire growth and smoke behavior is an important and historically difficult task. Here we compare a coupled fire‐weather model to current practices used in air quality forecasting in their ability to predict daily wildfire spread and fire intensity for the 2019 Williams Flats Fire. We also evaluate the fire‐weather model against high‐resolution satellite and aircraft measurements in ways previously unexplored. We find that including fire‐fighting efforts in our model makes the biggest improvements toward accurate wildfire forecasting. When we account for fire‐fighting efforts, fuel moisture maps, and increased fuel loads, our coupled fire‐weather model significantly outperforms simpler methods with reasonable computational time. Despite this, modeled fire intensity tends to lead observations by at least an hour. Optimal configuration options and avenues for forecasting improvements are discussed. Key Points: Adding containment lines into our wildfire model made the biggest difference in improving accuracy of daily burned area predictionsAccounting for containment, fuel moisture content maps, and increased fuel density consistently increased prediction skill above persistenceModeled fire radiative power leads observations by at least an hour, but with similar accuracy to prescribed diurnal cycles [ABSTRACT FROM AUTHOR]

Concentrations of ambient particulate matter (such as PM2.5 and PM10) have come to represent a serious environmental problem worldwide, causing many deaths and economic losses. Because of the detrimental effects of PM2.5 on human health, many countries and international organizations have developed and operated regional and global short-term PM2.5 prediction systems. The short-term predictability of PM2.5 (and PM10) is determined by two main factors: the performance of the air quality model and the precision of the initial states. While specifically focusing on the latter factor, this study attempts to demonstrate how information from classical ground observation networks, a state-of-the-art geostationary (GEO) satellite sensor, and an advanced air quality modeling system can be synergistically combined to improve short-term PM2.5 predictability over South Korea. Such a synergistic combination of information can effectively overcome the major obstacle of scarcity of information, which frequently occurs in PM2.5 prediction systems using low Earth orbit (LEO) satellite-borne observations. This study first presents that the scarcity of information is mainly associated with cloud masking, sun-glint effect, and ill-location of satellite-borne data, and it then demonstrates that an advanced air quality modeling system equipped with synergistically-combined information can achieve substantially improved performances, producing enhancements of approximately 10%, 19%, 29%, and 10% in the predictability of PM2.5 over South Korea in terms of index of agreement (IOA), correlation coefficient (R), mean biases (MB), and hit rate (HR), respectively, compared to PM2.5 prediction systems using only LEO satellite-derived observations. [ABSTRACT FROM AUTHOR]

Aerosol mass extinction efficiency (MEE) is a key aerosol property used to connect aerosol optical properties with aerosol mass concentrations. Using measurements of smoke obtained during the Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) campaign we find that mid‐visible smoke MEE can change by a factor of 2–3 between fresh smoke (<2 hr old) and one‐day‐old smoke. While increases in aerosol size partially explain this trend, changes in the real part of the aerosol refractive index (real(n)) are necessary to provide closure assuming Mie theory. Real(n) estimates derived from multiple days of FIREX‐AQ measurements increase with age (from 1.40 – 1.45 to 1.5–1.54 from fresh to one‐day‐old) and are found to be positively correlated with organic aerosol oxidation state and aerosol size, and negatively correlated with smoke volatility. Future laboratory, field, and modeling studies should focus on better understanding and parameterizing these relationships to fully represent smoke aging. Plain Language Summary: A common way to observe airborne particles produced by biomass burning is through aerosol optical properties, for instance, using aerosol optical depth from satellites or low‐cost sensors that measure scattered light. Since health effects are associated to aerosol mass concentrations, a conversion factor between them is needed. Here we use in‐plume measurements collected from an aircraft to show that aging processes alone can produce a factor of 2–3 change in aerosol extinction per unit of aerosol mass concentration. We also find that these changes are driven not only due to changes in aerosol size, but also due to changes in the material properties of aerosols. These results are relevant as fires are becoming more common and extreme, and thus these changes in smoke properties need to be taken into consideration in many fields of study such as assimilating satellite smoke into atmospheric composition models, satellite‐based smoke impacts on health, and corrections for low‐cost PM2.5 sensors. Key Points: Aerosol mass extinction efficiency can increase up to a factor of 2–3 after 1 day of agingChanges in both particle mean diameter and real part of the refractive index are needed to fully explain the changesChanges in the estimated real part of the refractive index are correlated to organic aerosol oxidation state, volatility, and particle size [ABSTRACT FROM AUTHOR]

The 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field experiment obtained a diverse set of in situ and remotely sensed measurements before and during a pyrocumulonimbus (pyroCb) event over the Williams Flats fire in Washington State. This unique dataset confirms that pyroCb activity is an efficient vertical smoke transport pathway into the upper troposphere and lower stratosphere (UTLS). The magnitude of smoke plumes observed in the UTLS has increased significantly in recent years, following unprecedented wildfire and pyroCb activity observed worldwide. The FIREX-AQ pyroCb dataset is therefore extremely relevant to a broad community, providing the first measurements of fresh smoke exhaust in the upper troposphere, including from within active pyroCb cloud tops. High-resolution remote sensing reveals that three plume cores linked to localized fire fronts, burning primarily in dense forest fuels, contributed to four total pyroCb "pulses." Rapid changes in fire geometry and spatial extent dramatically influenced the magnitude, behavior, and duration of pyroCb activity. Cloud probe measurements and weather radar identify the presence of large ice particles within the pyroCb and hydrometers below cloud base, indicating precipitation development. The resulting feedbacks suggest that vertical smoke transport efficiency was reduced slightly when compared with intense pyroCb events reaching the lower stratosphere. Physical and optical aerosol property measurements in pyroCb exhaust are compared with previous assumptions. A large suite of aerosol and gas-phase chemistry measurements sets a foundation for future studies aimed at understanding the composition of smoke plumes lifted by pyroconvection into the UTLS and their role in the climate system. [ABSTRACT FROM AUTHOR]

KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM 2.5 , often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m 2 g -1 observed average) and light-scattering enhancement factor (f (RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm -3 in the model vs. observed average of 1.5 g cm -3) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation. [ABSTRACT FROM AUTHOR]

For the purpose of improving PM prediction skills in East Asia, we estimated a new background error covariance matrix (BEC) for aerosol data assimilation using surface PM2.5 observations that accounts for the uncertainties in anthropogenic emissions. In contrast to the conventional method to estimate the BEC that uses perturbations in meteorological data, this method additionally considered the perturbations using two different emission inventories. The impacts of the new BEC were then tested for the prediction of surface PM2.5 over East Asia using Community Multi-scale Air Quality (CMAQ) initialized by three-dimensional variational method (3D-VAR). The surface PM2.5 data measured at 154 sites in South Korea and 1,535 sites in China were assimilated every six hours during the Korea-United States Air Quality Study (KORUS-AQ) campaign period (1 May-14 June 2016). Data assimilation with our new BEC showed better agreement with the surface PM2.5 observations than that with the conventional method. Our method also showed closer agreement with the observations in 24-hour PM2.5 predictions with ~ 44 % fewer negative biases than the conventional method. We conclude that increased standard deviations, together with horizontal and vertical length scales in the new BEC, tend to improve the data assimilation and short-term predictions for the surface PM2.5. This paper also suggests further research efforts devoted to estimating the BEC to improve PM2.5 predictions. [ABSTRACT FROM AUTHOR]

NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ, conducted in 2011–2014) campaign in the United States and the joint NASA and National Institute of Environmental Research (NIER) Korea–United States Air Quality Study (KORUS-AQ, conducted in 2016) in South Korea were two field study programs that provided comprehensive, integrated datasets of airborne and surface observations of atmospheric constituents, including nitrogen dioxide (NO2), with the goal of improving the interpretation of spaceborne remote sensing data. Various types of NO2 measurements were made, including in situ concentrations and column amounts of NO2 using ground- and aircraft-based instruments, while NO2 column amounts were being derived from the Ozone Monitoring Instrument (OMI) on the Aura satellite. This study takes advantage of these unique datasets by first evaluating in situ data taken from two different instruments on the same aircraft platform, comparing coincidentally sampled profile-integrated columns from aircraft spirals with remotely sensed column observations from ground-based Pandora spectrometers, intercomparing column observations from the ground (Pandora), aircraft (in situ vertical spirals), and space (OMI), and evaluating NO2 simulations from coarse Global Modeling Initiative (GMI) and high-resolution regional models. We then use these data to interpret observed discrepancies due to differences in sampling and deficiencies in the data reduction process. Finally, we assess satellite retrieval sensitivity to observed and modeled a priori NO2 profiles. Contemporaneous measurements from two aircraft instruments that likely sample similar air masses generally agree very well but are also found to differ in integrated columns by up to 31.9 %. These show even larger differences with Pandora, reaching up to 53.9 %, potentially due to a combination of strong gradients in NO2 fields that could be missed by aircraft spirals and errors in the Pandora retrievals. OMI NO2 values are about a factor of 2 lower in these highly polluted environments due in part to inaccurate retrieval assumptions (e.g., a priori profiles) but mostly to OMI's large footprint (>312 km 2). [ABSTRACT FROM AUTHOR]

NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign in the United States and the joint NASA and National Institute of Environmental Research (NIER) Korea-United States Air Quality Study (KORUS-AQ) in South Korea were two field study programs that provided comprehensive, integrated datasets of airborne and surface observations of atmospheric constituents, including nitrogen dioxide (NO2), with a goal of improving the interpretation of spaceborne remote sensing data. Various types of NO2 measurements were made, including in situ concentrations and column amounts of NO2 using ground- and aircraft-based instruments, while NO2 column amounts were being derived from the Ozone Monitoring Instrument (OMI) on the Aura satellite. This study takes advantage of these unique data sets by first evaluating in situ data taken from two different instruments on the same aircraft platform, comparing coincidently sampled profile-integrated columns from aircraft spirals with remotely sensed column observations from ground-based Pandora spectrometers, intercomparing column observations from the ground (Pandora), aircraft (in situ vertical spirals), and space (OMI), and evaluating NO2 simulations from coarse Global Modeling Initiative (GMI) and high-resolution regional models. We then use these data to interpret observed discrepancies due to differences in sampling and deficiencies in the data reduction process. Finally, we assess satellite retrieval sensitivity to observed and modeled a-priori NO2 profiles. Contemporaneous measurements from two aircraft instruments that likely sample similar air masses generally agree very well but are also found to differ in integrated columns by up to 33.3%. These show even larger differences with Pandora, reaching up to 53.1%, potentially due to a combination of strong gradients in NO2 fields that could be missed by aircraft spirals and errors in the Pandora retrievals. OMI NO2 values are about a factor of two lower in these highly polluted environments, due in part to inaccurate retrieval assumptions (e.g., a priori profiles), but mostly to OMI's areal (> 312 km²) averaging. [ABSTRACT FROM AUTHOR]

Recently launched multichannel geostationary Earth orbit (GEO) satellite sensors, such as the Geostationary Ocean Color Imager (GOCI) and the Advanced Himawari Imager (AHI), provide aerosol products over East Asia with high accuracy, which enables the monitoring of rapid diurnal variations and the transboundary transport of aerosols. Most aerosol studies to date have used low Earth orbit (LEO) satellite sensors, such as the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging Spectroradiometer (MISR), with a maximum of one or two overpass daylight times per day from midlatitudes to low latitudes. Thus, the demand for new GEO observations with high temporal resolution and improved accuracy has been significant. In this study the latest versions of aerosol optical depth (AOD) products from three LEO sensors – MODIS (Dark Target, Deep Blue, and MAIAC), MISR, and the Visible/Infrared Imager Radiometer Suite (VIIRS), along with two GEO sensors (GOCI and AHI), are validated, compared, and integrated for a period during the Korea–United States Air Quality Study (KORUS-AQ) field campaign from 1 May to 12 June 2016 over East Asia. The AOD products analyzed here generally have high accuracy with high R (0.84–0.93) and low RMSE (0.12–0.17), but their error characteristics differ according to the use of several different surface-reflectance estimation methods. High-accuracy near-real-time GOCI and AHI measurements facilitate the detection of rapid AOD changes, such as smoke aerosol transport from Russia to Japan on 18–21 May 2016, heavy pollution transport from China to the Korean Peninsula on 25 May 2016, and local emission transport from the Seoul Metropolitan Area to the Yellow Sea in South Korea on 5 June 2016. These high-temporal-resolution GEO measurements result in more representative daily AOD values and make a greater contribution to a combined daily AOD product assembled by median value selection with a 0.5∘×0.5∘ grid resolution. The combined AOD is spatially continuous and has a greater number of pixels with high accuracy (fraction within expected error range of 0.61) than individual products. This study characterizes aerosol measurements from LEO and GEO satellites currently in operation over East Asia, and the results presented here can be used to evaluate satellite measurement bias and air quality models. [ABSTRACT FROM AUTHOR]

This study develops a new approach to improve simulations of the particulate matter of aerodynamic diameter smaller than 2.5 μm (PM2.5) in the Community Multiscale Air Quality (CMAQ) model via assimilation of Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) retrievals using the Gridpoint Statistical Interpolation (GSI) system. In contrast to previous studies that only consider errors due to transport, our computation of the background error covariance matrix incorporates uncertainties in anthropogenic emissions. To understand the impact of this approach, three experiments (one background and two assimilations) are performed over the contiguous United States (CONUS) from 15 July to 14 August 2014. The background CMAQ experiment significantly underestimates both the MODIS AOD and surface PM2.5 levels. MODIS AOD assimilation pushes both the CMAQ AOD and surface PM2.5 distributions toward the observed distributions, but CMAQ still underestimates the observations. Averaged over CONUS, the two assimilation experiments with and without including the anthropogenic emission uncertainties improve the correlation coefficient between the model and independent observations of PM2.5 by ~67% and ~48%, respectively, and reduces the mean bias by ~38% and ~10%, respectively. The assimilation improves the model performance everywhere over CONUS, except the New York and Wisconsin, where CMAQ overestimates the observed PM2.5 during nighttime after assimilation likely because of overcorrection of aerosol mass concentrations by the AOD assimilation. Future work should incorporate uncertainties in other processes (biomass burning and biogenic emissions, deposition, chemistry, transport, and boundary conditions) to further enhance the value of assimilating spaceborne AOD retrievals. Key Points: Assimilation of MODIS AOD retrievals in CMAQ via GSI to improve surface PM2.5 forecastsAccounting for uncertainties in anthropogenic emissions significantly improves the model performance after data assimilationThe assimilation‐induced improvements in CMAQ aerosol initial conditions last for more than 48 hr [ABSTRACT FROM AUTHOR]

Recently launched multi-channel geostationary-Earth-orbit (GEO) satellite sensors such as the Geostationary Ocean Color Imager (GOCI) and the Advanced Himawari Imager (AHI) provide aerosol products over East Asia with high accuracy, which enables the monitoring of rapid diurnal variations and the transboundary transport of aerosols. Most aerosol studies to date have used low-Earth-orbit (LEO) satellite sensors, such as the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging SpectroRadiometer (MISR) with a maximum of one or two overpass daylight times per day at mid- to low latitudes. Thus, the demand for new GEO observations with high temporal resolution and improved accuracy has been significant. In this study the aerosol optical depth (AOD) products from three LEO sensors – MODIS, MISR, and the Visible/Infrared Imager Radiometer Suite (VIIRS) – along with two GEO sensors – GOCI and AHI – are validated, compared and integrated for the period during the Korea–United Sates Air Quality Study (KORUS-AQ) field campaign from 1 May to 12 June 2016 over East Asia. The AOD products analyzed here generally have high accuracy, but their error characteristics differ according to the use of several different surface-reflectance estimation methods plus differences in cloud screening. High-accuracy near-real-time GOCI and AHI measurements facilitate the detection of rapid AOD changes, such as smoke aerosol transport from Russia to Japan on 18–21 May 2016, heavy pollution transport from China to Korea on 25 May 2016, and local emission transport from the Seoul Metropolitan Area to the Yellow Sea in Korea on 5 June 2016. These high-temporal-resolution GEO measurements result in more-representative daily AOD values and make a greater contribution to a combined daily AOD product assembled by median-value selection with a 0.5° × 0.5° grid resolution. The combined AOD is more spatially continuous and of higher accuracy than the individual products. This study characterizes aerosol measurements from LEO and GEO satellites currently in operation over East Asia, and results presented here can be used to evaluate satellite measurement bias and air-quality models. [ABSTRACT FROM AUTHOR]

In this work, we investigate the NOx emissions inventory in Seoul, South Korea, using a regional ozone monitoring instrument (OMI) NO2 product derived from the standard NASA product. We first develop a regional OMI NO2 product by recalculating the air mass factors using a high-resolution (4 km × 4 km) WRF-Chem model simulation, which better captures the NO2 profile shapes in urban regions. We then apply a model-derived spatial averaging kernel to further downscale the retrieval and account for the subpixel variability. These two modifications yield OMI NO2 values in the regional product that are 1.37 times larger in the Seoul metropolitan region and >2 times larger near substantial point sources. These two modifications also yield an OMI NO2 product that is in better agreement with the Pandora NO2 spectrometer measurements acquired during the South Korea–United States Air Quality (KORUS-AQ) field campaign. NOx emissions are then derived for the Seoul metropolitan area during the KORUS-AQ field campaign using a top-down approach with the standard and regional NASA OMI NO2 products. We first apply the top-down approach to a model simulation to ensure that the method is appropriate: the WRF-Chem simulation utilizing the bottom-up emissions inventory yields a NOx emissions rate of 227±94 kt yr -1 , while the bottom-up inventory itself within a 40 km radius of Seoul yields a NOx emissions rate of 198 kt yr -1. Using the top-down approach on the regional OMI NO2 product, we derive the NOx emissions rate from Seoul to be 484±201 kt yr -1 , and a 353±146 kt yr -1 NOx emissions rate using the standard NASA OMI NO2 product. This suggests an underestimate of 53 % and 36 % in the bottom-up inventory using the regional and standard NASA OMI NO2 products respectively. To supplement this finding, we compare the NO2 and NOy simulated by WRF-Chem to observations of the same quantity acquired by aircraft and find a model underestimate. When NOx emissions in the WRF-Chem model are increased by a factor of 2.13 in the Seoul metropolitan area, there is better agreement with KORUS-AQ aircraft observations and the recalculated OMI NO2 tropospheric columns. Finally, we show that by using a WRF-Chem simulation with an updated emissions inventory to recalculate the air mass factor (AMF), there are small differences (∼8 %) in OMI NO2 compared to using the original WRF-Chem simulation to derive the AMF. This suggests that changes in model resolution have a larger effect on the AMF calculation than modifications to the South Korean emissions inventory. Although the current work is focused on South Korea using OMI, the methodology developed in this work can be applied to other world regions using TROPOMI and future satellite datasets (e.g., GEMS and TEMPO) to produce high-quality region-specific top-down NOx emissions estimates. [ABSTRACT FROM AUTHOR]

Spatial distribution of diurnal variations of aerosol properties in South Korea, both long term and short term, is studied by using 9 AERONET (AErosol RObotic NETwork) sites from 1999 to 2017 and an additional 10 sites during the KORUS-AQ (Korea--United States Air Quality) field campaign in May and June of 2016. The extent to which the WRF-Chem (Weather Research and Forecasting coupled with Chemistry) model and the GOCI (Geostationary Ocean Color Imager) satellite retrieval can describe these variations is also analyzed. On a daily average, aerosol optical depth (AOD) at 550 nm is 0.386 and shows a diurnal variation of 20 to - 30% in inland sites, which is larger than the AOD of 0.308 and diurnal variation of -20% seen in coastal sites. For all the inland and coastal sites, AERONET, GOCI, and WRF-Chem, and observed PM2.5 (particulate matter with aerodynamic diameter less than 2.5 µm) data generally show dual peaks for both AOD and PM2.5, one in the morning (often at ~ 08.00-10.00 KST, Korea Standard Time, especially for PM2.5/ and another in the early afternoon (~ 14:00 KST, albeit for PM2.5 this peak is smaller and sometimes insignificant). In contrast, Ångström exponent values in all sites are between 1.2 and 1.4 with the exception of the inland rural sites having smaller values near 1.0 during the early morning hours. All inland sites experience a pronounced increase in the Ångström exponent from morning to evening, reflecting an overall decrease in particle size in daytime. To statistically obtain the climatology of diurnal variation of AOD, a minimum requirement of ~ 2 years of observation is needed in coastal rural sites, twice as long as that required for the urban sites, which suggests that the diurnal variation of AOD in an urban setting is more distinct and persistent. While Korean GOCI satellite retrievals are able to consistently capture the diurnal variation of AOD (although it has a systematically low bias of 0.04 on average and up to 0.09 in later afternoon hours), WRF-Chem clearly has a deficiency in describing the relative change of peaks and variations between the morning and afternoon, suggesting further studies for the diurnal profile of emissions. Furthermore, the ratio between PM2.5 and AOD in WRF-Chem is persistently larger than the observed counterparts by 30 %-50% in different sites, but spatially no consistent diurnal variation pattern of this ratio can be found. Overall, the relatively small diurnal variation of PM2.5 is in high contrast with large AOD diurnal variation, which suggests the large diurnal variation of AOD-PM2.5 relationships (with the PM2.5 =AOD ratio being largest in the early morning, decreasing around noon, and increasing in late afternoon) and, therefore, the need to use AOD from geosta [ABSTRACT FROM AUTHOR]

The Gridpoint Statistical Interpolation (GSI) Three-Dimensional Variational (3DVAR) data assimilation system is extended to treat the MOSAIC aerosol model in WRF-Chem, and to be capable of assimilating surface PM2.5 concentrations. The coupled GSI-WRF-Chem system is applied to reproduce aerosol levels over China during an extremely polluted winter month, January 2013. After assimilating surface PM2.5 concentrations, the correlation coefficients between observations and model results averaged over the assimilated sites are improved from 0.67 to 0.94. At nonassimilated sites, improvements (higher correlation coefficients and lower mean bias errors (MBE) and root-mean-square errors (RMSE)) are also found in PM2.5, PM10, and AOD predictions. Using the constrained aerosol fields, we estimate that the PM2.5 concentrations in January 2013 might have caused 7550 premature deaths in Jing-Jin-Ji areas, which are 2% higher than the estimates using unconstrained aerosol fields. We also estimate that the daytime monthly mean anthropogenic aerosol radiative forcing (ARF) to be -29.9W/m² at the surface, 27.0W/m² inside the atmosphere, and -2.9W/m² at the top of the atmosphere. Our estimates update the previously reported overestimations along Yangtze River region and underestimations in North China. This GSI-WRF-Chem system would also be potentially useful for air quality forecasting in China. [ABSTRACT FROM AUTHOR]

Limitations in current capabilities to constrain aerosols adversely impact atmospheric simulations. Typically, aerosol burdens within models are constrained employing satellite aerosol optical properties, which are not available under cloudy conditions. Here we set the first steps to overcome the long-standing limitation that aerosols cannot be constrained using satellite remote sensing under cloudy conditions. We introduce a unique data assimilation method that uses cloud droplet number (Wd) retrievals to improve predicted below-cloud aerosol mass and number concentrations. The assimilation, which uses an adjoint aerosol activation parameterization, improves agreement with independent Nd observations and with in situ aerosol measurements below shallow cumulus clouds. The impacts of a single assimilation on aerosol and cloud forecasts extend beyond 24 h. Unlike previous methods, this technique can directly improve predictions of near-surface fine mode aerosols responsible for human health impacts and low-cloud radiative forcing. Better constrained aerosol distributions will help improve health effects studies, atmospheric emissions estimates, and airquality, weather, and climate predictions. [ABSTRACT FROM AUTHOR]

To improve PM 2.5 predictions in Northeast Asia, we estimated a new background error covariance matrix (BEC) for aerosol data assimilation using surface PM 2.5 observations. In contrast to the conventional method of BEC estimation that uses perturbations in meteorological data, this method additionally considered the perturbations using two different emission inventories. By taking the emission uncertainty into account, we found that the standard deviations in the BEC were significantly increased. The standard deviations became around three times larger than those in the conventional method at the surface. The impacts of the new BEC were then tested for the prediction of surface PM 2.5 over Northeast Asia using the Community Multiscale Air Quality (CMAQ) model initialized by three-dimensional variational method (3D-VAR). The surface PM 2.5 data measured at 154 sites in South Korea and 1535 sites in China were assimilated every 6 h during the campaign period of the Korea-United States Air Quality Study (KORUS-AQ) (1 May–14 June 2016). The data assimilation with the new BEC showed better agreement with the surface PM 2.5 observations than with the BEC from the conventional method. Our method was also more consistent with the observations in 24-h PM 2.5 predictions than the conventional method (specifically, with a ∼44% reduction of negative biases). We concluded that increased standard deviations, together with updated horizontal and vertical length scales in the new BEC, improved the data assimilation and short-term predictions of the surface PM 2.5. This paper also suggests several research efforts to further improve the BEC for better short-term PM 2.5 predictions in Northeast Asia. [Display omitted] • A new background error covariance (BEC) for PM 2.5 predictions was developed. • The new BEC considers the uncertainties in anthropogenic emissions. • Two different emission inventories were used to account for the uncertainty. • 24-h PM 2.5 predictions were improved with ∼44% fewer negative biases. [ABSTRACT FROM AUTHOR]